Theoretical Investigation on The Partial Oxidation of Methane to Methanol and Methanol to Formaldehyde or Methanediol Using Transition Metal Oxide Anions

Abstract

In this thesis, theoretical calculations were made to study three important processes as follows: 1) Methane to methanol conversion 2) Methanol to formaldehyde conversion 3) Methanol to methanediol conversion. For these processes, different step-by-step reaction mechanisms were explicitly considered. All the generated structures were in complete agreement with the expectations made for them, and the optimized energy and vibrational frequencies for each structure were explicitly calculated. The energy profile for each process was built by taking into consideration the calculated electronic energy for each structure. A comparison between each catalytic path was made to determine the one with the lowest energy barriers aiming to select the path by which the reaction will proceed. Metal oxide anions were used in the gas phase as catalysts in each of those conversion processes, focusing on nickel and palladium oxides. All the calculations made for each process were finalized using the MN15 method with correlation-consistent basis sets of triple-ζ quality. The results confirm that both nickel and palladium oxide anions are good candidates for any of the conversion processes listed above. The thesis strongly suggests using metal oxide anions of transition elements for future chemical reactions whether as catalysts or reacting molecules.